Strongly Quantum-Confined Blue-Emitting Excitons in Chemically Configurable Multiquantum Wells

Kaiyuan Yao, Mary S. Collins, Kara M. Nell, Edward S. Barnard, Nicholas J. Borys, Tevye Kuykendall, J. Nathan Hohman, P. James Schuck

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Light matter interactions are greatly enhanced in two-dimensional (2D) semiconductors because of strong excitonic effects. Many optoelectronic applications would benefit from creating stacks of atomically thin 2D semiconductors separated by insulating barrier layers, forming multiquantum-well structures. However, most 2D transition metal chalcogenide systems require serial stacking to create van der Waals multilayers. Hybrid metal organic chalcogenolates (MOChas) are self-assembling hybrid materials that combine multiquantum-well properties with scalable chemical synthesis and air stability. In this work, we use spatially resolved linear and nonlinear optical spectroscopies over a range of temperatures to study the strongly excitonic optical properties of mithrene, that is, silver benzeneselenolate, and its synthetic isostructures. We experimentally probe s-type bright excitons and p-type excitonic dark states formed in the quantum confined 2D inorganic monolayers of silver selenide with exciton binding energy up to ∼0.4 eV, matching recent theoretical predictions of the material class. We further show that mithrene's highly efficient blue photoluminescence, ultrafast exciton radiative dynamics, as well as flexible tunability of molecular structure and optical properties demonstrate great potential of MOChas for constructing optoelectronic and quantum excitonic devices.

Original languageEnglish (US)
Pages (from-to)4085-4092
Number of pages8
JournalACS nano
Volume15
Issue number3
DOIs
StatePublished - Nov 9 2020

Bibliographical note

Funding Information:
The authors thank T. E. Smidt, J. B. Neaton, and A. Schwartzberg for discussions. This work is supported by Programmable Quantum Materials, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Award No. DE-SC0019443. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Publisher Copyright:
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Keywords

  • exciton
  • hybrid semiconductor
  • mithrene
  • photoluminescence
  • quantum well
  • self-assembly
  • van der Waals heterostructure

PubMed: MeSH publication types

  • Journal Article

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